Computational screening of core@shell nanoparticles for the hydrogen evolution and oxygen reduction reactions

Corona, Benjamin T.; Howard, Marco D.; Zhang, Liang; Henkelman, Graeme

doi:10.1063/1.4972579

Cited by 23 publications

(16 citation statements)

References 21 publications

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“…Recently nanoframes of Pt 3 Ni 17 and Pt–Ru–M (M = Ni, Fe, or Co) alloys 18 have shown extraordinary results outperforming Pt alone, but Pt remains the basic component of these multi-metallic nanoparticles. In electrocatalysis, density functional theory (DFT) predicts better results for Pt skins 19 , 20 . The use of Pt skins substantially reduces the amount of Pt, but introduces new problems such as difficulties in manipulating the nanoscale elemental distribution 21 and the surface segregation of Pt.…”

Section: Introductionmentioning

confidence: 99%

Synergistic effect of nano-Pt and Ni spine for HER in alkaline solution: hydrogen spillover from nano-Pt to Ni spine

Abbas

Kim

Iqbal

et al. 2018

Sci Rep

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The design of active, stable, and cost-effective electrocatalysts for the H2 evolution reaction (HER) in alkaline conditions is important for electrochemical systems such as the chloro-alkaline process and H2 production. Here we report catalysts comprising Pt on Ni single crystalline spines (Pt/Ni-SP) with high activity and stability for HER in alkaline solution with proposed mechanism. The Pt/Ni-SP catalysts are prepared by dispersing platinum nanoparticles (1.7–3.1 nm) on the single-crystalline spines (Ni-SP) of Ni urchin-like particles. The size and coverage of Pt nanoparticles on Ni-SP are increased with increases in the Pt loading amount. X-ray diffraction, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy are performed to observe the structure of the Pt/Ni-SP catalyst. The catalysts achieve the mass activity of 1.11 A mg−1(Pt), comparing favorably to Pt/C catalysts with the mass activity of 0.33 A mg−1(Pt) at 0.05 V overpotential. The Tafel slope of the Pt/Ni-SP catalyst is approximately 30 mV dec−1, similar to that of Pt, while Pt/Ni-SP is very stable in alkaline solution, like Ni. The synergistic effect of Pt/Ni-SP is ascribed to H spillover from Pt to Ni.

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Section: Introductionmentioning

confidence: 99%

Synergistic effect of nano-Pt and Ni spine for HER in alkaline solution: hydrogen spillover from nano-Pt to Ni spine

Abbas

Kim

Iqbal

et al. 2018

Sci Rep

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“…Based on the volcano plot, it was suggested that the best ORR catalysts should bind *OH slightly weaker (0.1–0.2 eV) than Pt(1 1 1) (highlighted in white in Figure C), and this has been a main framework toward a massive computational screening to develop improved ORR catalysts. Indeed, there are many examples of high‐throughput screening for active ORR catalysts in the literature on this basis . However, we emphasize that the use of the volcano plot with Δ G (*OH) as a single descriptor is valid only if the scaling relation among *O, *OH, and *OOH holds.…”

Section: Resultsmentioning

confidence: 99%

Importance of Ligand Effects Breaking the Scaling Relation for Core–Shell Oxygen Reduction Catalysts

Back

Jung

2017

ChemCatChem

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Tremendous recent efforts have been made toward developing highly active oxygen reduction reaction (ORR) catalysts with a minimized usage of noble metal Pt by using Pt alloys and core–Pt shell structures. A main computational framework for such a goal has been the search for a new material with the *OH binding slightly weaker than Pt based on the conventional volcano relation of ORR activity versus *OH binding energy. In this work, by using carbides and nitrides as core materials, we demonstrate that the conventional scaling relation between *OH and *O can be completely broken owing to a significant ligand–Pt orbital interactions in the core–Pt shell structure, and in such cases, the usual catalyst design strategy of tuning the *OH binding energy of Pt to a weaker leg of the volcano can mislead the prediction. In these cases, one needs to consider all reaction intermediates to appropriately predict the activity of ORR catalysts. We additionally show that, although the transition metal nitrides and carbides studied here as core materials all induce an undesired tensile strain to the Pt overlayers with a stronger *OH binding, a proper tuning of the ligand (core) effects in the Pt1 and Pt2 overlayers core–shell configurations can lead to an activity comparable to or slightly better than Pt.

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“…In addition, computational calculations of Jiang et al [50] showed partial charge transfer from Ni to Pt in Pt m Ni n alloy clusters, which was supposed to be responsible for the decreased CO poisoning. On the other hand, Corona et al [32] reported the binding energy tuning of oxygen species with Pt for Pt(Ni) core-shell structures, thus increasing the activity for the oxygen reduction reaction. As a result, Ni in Pt(Ni) produces a positive effect in increasing the CO tolerance of Pt.…”

Section: Co Electrooxidationmentioning

confidence: 99%

“…At present, the benchmark catalysts for PEMFCs in the industrial-related applications are carbon-supported Pt and Pt-based alloys [28]. It is generally accepted that alloying Pt with other transition metals allows improving the reaction rates by tuning the d-band structure of the Pt surfaces to lower the bond strength of the Pt-adsorbates, thus leading to better resistance to poisoning [12,[28][29][30][31][32]. Many basic research scientists are currently focusing their attention to obtain catalysts with precursors that provide good electrocatalytic activity using small amounts of noble catalytic metals to lower costs [33][34][35][36].…”

Section: Introductionmentioning

confidence: 99%

Synthesis and Evaluation of PtNi Electrocatalysts for CO and Methanol Oxidation in Low Temperature Fuel Cells

et al. 2020

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Pt(Ni)/C and PtRu(Ni)/C catalysts were synthesized by electroless deposition of Ni on a carbon dispersion followed by sequenced Pt deposition and spontaneous deposition of Ru species. The structural analyses of the catalysts with 88:12 and 98:2 Pt:Ni atomic ratios pointed out to the formation of small hexagonal Ni crystallites covered by thin cubic Pt surface structures with no evidence about PtNi alloy formation. The onset potentials for CO oxidation on Pt(Ni)/C and PtRu(Ni)/C were about 0.10 and 0.24 V more negative than those of Pt/C, thus indicating their better CO tolerance. The surface Ru species appeared to have the major effect by facilitating the CO removal by the bifunctional mechanism. The onset potential for the methanol oxidation reaction (MOR) of Pt(Ni)/C was about 0.15 V lower than that of Pt/C. The mass and specific activities together with the exchange current densities of the Pt(Ni)/C catalysts were also higher than those of Pt/C, making in evidence their higher activity in front of the MOR. The Tafel slopes for the MOR on Pt(Ni)/C suggested different reaction mechanism than on Pt/C. The electronic (ligand) effect of Ni on Pt was considered the main reason to explain the higher activity of Pt(Ni)/C in front of the CO oxidation and the MOR.

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Computational screening of core@shell nanoparticles for the hydrogen evolution and oxygen reduction reactions

Cited by 23 publications

References 21 publications

Synergistic effect of nano-Pt and Ni spine for HER in alkaline solution: hydrogen spillover from nano-Pt to Ni spine

Synergistic effect of nano-Pt and Ni spine for HER in alkaline solution: hydrogen spillover from nano-Pt to Ni spine

Importance of Ligand Effects Breaking the Scaling Relation for Core–Shell Oxygen Reduction Catalysts

Synthesis and Evaluation of PtNi Electrocatalysts for CO and Methanol Oxidation in Low Temperature Fuel Cells

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